One-Step Synthesis of Dimethyl Ether from Syngas with Fe-Modified Zeolite ZSM-5 as Dehydration Catalyst

Xia, Jianchao; Mao, Dongsen; Zhang, Bin; Chen, Qingling; Tang, Yi

doi:10.1007/s10562-004-8686-x

Cited by 70 publications

(42 citation statements)

References 22 publications

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“…Kinetic models (5), (6), (11) and (13) have been presented in typical categories, i.e., according to the level of changes of the solid phase (a s ) or of CO 2 (a) or share of the gas phase constituents ([CO], [CO 2 ]) with time. The research presented was intended for another objective because the authors were interested in the influence of pressure on the gasification process by means of CO 2 .…”

Section: Resultsmentioning

confidence: 99%

“…The stand has been used to determine the fuels' reactivity in conditions of elevated pressure as high as 5 MPa. Carbon dioxide is supplied from the bottle through a reduction valve (1) at the established flowrate, set by means of the controller (3), to the pressure pipe reactor (6) placed vertically in an electric oven (4). In the initial zone of the reactor (6), filled in with the ceramic balls to increase thermal capacity of the system, carbon dioxide is heated up to the required temperature.…”

Section: Methodsmentioning

confidence: 99%

“…Carbon monoxide can be applied in many chemical synthesis reactions [3][4][5][6][7][8] including the following:…”

Section: Introductionmentioning

confidence: 99%

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The Boudouard–Bell reaction analysis under high pressure conditions

Mianowski

Robak

Tomaszewicz

et al. 2012

J Therm Anal Calorim

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A new method for the measurement of solid fuel reactivity towards carbon dioxide has been developed. This new method takes into account high-pressure and temperature effects. Three devolatilized carbonaceous materials have been used in experiments: chars derived from lignite, bituminous coal and blast furnace coke. Processes were carried out at temperatures of 800, 850 and 900°C and pressures of 1.52, 2.5 and 3.4 MPa. Analysis of the product gas composition was carried out with the maximum degree of conversion of CO 2 (a m ) proposed as a representative reactivity parameter. Arrhenius and Eyring relationships have been analyzed, and values of the activation energy and activation volume have been calculated.

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Section: Resultsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

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The Boudouard–Bell reaction analysis under high pressure conditions

Mianowski

Robak

Tomaszewicz

et al. 2012

J Therm Anal Calorim

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“…Furthermore, zeolites are more resistant than -Al 2 O 3 towards poisoning of acid sites by the water by-product [4,5,6]. Among the zeolites, the medium pore ZSM-5 (MFI) has been by far the most widely applied as the acid component in bifunctional DME synthesis catalysts [5,7,8,9,10,11], though other zeolites such as ferrierite, MCM-22 and its delaminated counterpart ITQ-2, IM-5, and TNU-9 have also been investigated [12,13].…”

Section: Introductionmentioning

confidence: 99%

The influence of zeolite surface-aluminum species on the deactivation of CuZnAl/zeolite hybrid catalysts for the direct DME synthesis

García‐Trenco

Martı́nez

2014

Catalysis Today

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ElsevierGarcía Martinez Feliu, A. (2014). The influence of zeolite surface-aluminum species on the deactivationof CuZnAl/zeolite hybrid catalysts for the direct DME synthesis. Catalysis Today. 227:144-153. doi:10.1016Today. 227:144-153. doi:10. /j.cattod.2013 AbstractIn this work, an original approach for preparing Cu-ZnO+H-ZSM-5 (Si/Al=15, denoted as Z5) hybrid catalysts displaying enhanced stability during the direct DME synthesis from syngas is presented. The adopted preparation strategy was based on the effective confinement of the copper catalyst within the pores of an SBA-15 silica carrier (d pore = 7.0 nm) prior to mixing with the acid zeolite. In order to maximize the Cu-ZnO interface area (where active Cu 0 sites are likely located) the walls of the SBA-15 silica were coated with a near-monolayer of ZnO (17 wt% Zn) prior the incorporation of copper (in concentrations of 10, 15, and 20 wt%) by the so-called ammonia-driving deposition-precipitation (ADP) method. Copper nanoparticles sizing 5-6 nm after H 2 -reduction (HRTEM) were effectively confined inside the SBA-15 mesopores (as supported by HAADF-STEM) for Cu loadings of up to 15 wt%. Higher Cu loadings (20 wt%) lead to large, XRD-visible, CuO nanoparticles residing out of the SBA-15 pores. The confined catalyst loaded with 15 wt% Cu (15Cu/Zn@S15) displayed the highest Cu 0 surface area (determined by N 2 O-RFC) and methanol synthesis activity. Then, hybrid catalysts based on this methanol synthesis function (15Cu/Zn@S15+Z5) were prepared in a 15Cu/Zn@S15:Z5 mass ratio of 2:1 by two methods: a) grinding the mixture of powders prior to pelletizing (method G), and b) mixing the pre-pelletized components (method M). Equivalent hybrids comprising a conventional coprecipitated Cu-ZnO-Al 2 O 3 (CZA) catalyst were also prepared for comparative purposes (CZA+Z5). The catalysts were evaluated for direct DME synthesis (533 K, 4.0 MPa) in runs lasting ca. 24 h. It was found that the confined 15Cu/Zn@S15+Z5 hybrids deactivated at a much lower rate than those based on CZA regardless the method of preparation. In turn, while conventional CZA+Z5 catalysts prepared by grinding (G) experienced a higher deactivation than that obtained by mixing (M) due to the contribution of detrimental interactions between the copper and zeolite components in the former, no differences in the deactivation rate were observed for the 15Cu/Zn@S15+Z5 hybrids prepared by grinding and mixing. The improved stability of these hybrid catalysts is accounted for by the inhibition of both detrimental interactions (by avoiding the direct contact of copper active sites and the zeolite surface) and extensive metal sintering (by limiting the extent of Cu 0 crystal growth) induced by the effective confinement of the Cu-based catalyst within the SBA-15 pores.

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“…In the latter process, first natural gas is reformed to synthesis gas, and then synthesis gas is converted into methanol or directly to DME. Synthesis of DME from synthesis gas (i.e., CO and H 2 ) is thermodynamically and economically more favorable than from methanol (Yaripour et al 2005;Brown et al 1991;Fei et al 2004;Qi et al 2001;Takeguchi et al 2000;Li et al 1996Li et al , 1997Ge et al 1998;Xia et al 2004;Ramos et al 2005;Jun et al 2003;Arena et al 2007;Liu et al 2001;Suh et al 2000;Sun et al 2003).…”

Section: Introductionmentioning

confidence: 99%

Direct production of dimethyl ether from synthesis gas utilizing bifunctional catalysts

2011

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In this study, direct synthesis of dimethyl ether from synthesis gas was investigated. For this purpose, H-mordenite zeolite was modified by wet impregnation of aluminum oxide onto it. The prepared catalysts were characterized by AAS, XRD and NH 3 -TPD analyses. Results of catalytic tests indicated that H-mordenite modified with 8 wt% aluminum oxide was an appropriate catalyst for synthesis of dimethyl ether (DME) from methanol in which methanol conversion and DME selectivity were 99.8 and 96.8%, respectively, without a noticeable change in catalyst stability. A series of bifunctional catalysts, CuZnO-ZrO 2 /Al-modified H-mordenite, were prepared by coprecipitating sedimentation method and characterized. Synthesis of DME via direct CO hydrogenation was then evaluated in a three-phase slurry reactor. Experimental results showed that Cu-ZnO-ZrO 2 /Al-modified H-mordenite was a suitable catalyst for the production of dimethyl ether from synthesis gas. Ultimately, the effects of operating conditions such as temperature, pressure and feed flow rate on the process performance of the determined optimum bifunctional catalyst have been reported.

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One-Step Synthesis of Dimethyl Ether from Syngas with Fe-Modified Zeolite ZSM-5 as Dehydration Catalyst

Cited by 70 publications

References 22 publications

The Boudouard–Bell reaction analysis under high pressure conditions

The Boudouard–Bell reaction analysis under high pressure conditions

The influence of zeolite surface-aluminum species on the deactivation of CuZnAl/zeolite hybrid catalysts for the direct DME synthesis

Direct production of dimethyl ether from synthesis gas utilizing bifunctional catalysts

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